Age-related cognitive decline brings decreases in functional status. Dispositional mindfulness, the tendency towards present-moment attention, is hypothesized to correspond with enhanced attention, whereas mind-wandering may be detrimental to cognition. The relationships among mindfulness, task-related and task-unrelated thought, and attentional control performance on Go/No-Go and Continuous Performance tasks were examined in older adults. Dispositional mindfulness was negatively associated with task-unrelated thought and was positively associated with reactive control, but not proactive control or Go/No-Go performance. Although mind-wandering was not directly associated with performance, task-unrelated thought mediated the mindfulness-proactive control relation. Fewer task-unrelated thoughts were associated with lower proactive control. Interestingly, this effect was moderated by working memory such that it was present for those with low-average, but not high, working memory. This study highlights the importance of dispositional mindfulness and mind-wandering propensity in accounting for individual differences in attentional control in older adults, providing important targets for future cognitive remediation interventions.